Key Laboratory of Analytical Science for Food Safety and Biology (MOE & Fujian Province), Department of Chemistry, Fuzhou University, Fuzhou 350108, People's Republic of China.
National Engineering Research Center for Carbohydrate Synthesis, Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, Key Laboratory for Green Chemistry of Jiangxi Province, Department of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, People's Republic of China.
ACS Sens. 2024 May 24;9(5):2684-2694. doi: 10.1021/acssensors.4c00621. Epub 2024 May 1.
Semiconductor-based photoelectrochemical (PEC) test protocols offer a viable solution for developing efficient individual health monitoring by converting light and chemical energy into electrical signals. However, slow reaction kinetics and electron-hole complexation at the interface limit their practical application. Here, we reported a triple-engineered CdS nanohierarchical structures (CdS NHs) modification scheme including morphology, defective states, and heterogeneous structure to achieve precise monitoring of the neurotransmitter dopamine (DA) in plasma and noninvasive body fluids. By precisely manipulating the Cd-S precursor, we achieved precise control over ternary CdS NHs and obtained well-defined layered self-assembled CdS NHs through a surface carbon treatment. The integration of defect states and the thin carbon layer effectively established carrier directional transfer pathways, thereby enhancing interface reaction sites and improving the conversion efficiency. The CdS NHs microelectrode fabricated demonstrated a remarkable negative response toward DA, thereby enabling the development of a miniature self-powered PEC device for precise quantification in human saliva. Additionally, the utilization of density functional theory calculations elucidated the structural characteristics of DA and the defect state of CdS, thus establishing crucial theoretical groundwork for optimizing the polymerization process of DA. The present study offers a potential engineering approach for developing high energy conversion efficiency PEC semiconductors as well as proposing a novel concept for designing sensitive testing strategies.
基于半导体的光电化学（PEC）测试协议通过将光和化学能转化为电信号，为开发高效的个体健康监测提供了可行的解决方案。然而，在界面处的反应动力学缓慢和电子-空穴复合限制了它们的实际应用。在这里，我们报告了一种三重工程化的 CdS 纳米分级结构（CdS NHs）修饰方案，包括形态、缺陷态和异质结构，以实现对神经递质多巴胺（DA）在血浆和非侵入性体液中的精确监测。通过精确操纵 Cd-S 前体，我们实现了对三元 CdS NHs 的精确控制，并通过表面碳处理获得了具有良好定义层状自组装 CdS NHs。缺陷态和薄碳层的集成有效地建立了载流子定向转移途径，从而增加了界面反应位点并提高了转换效率。所制备的 CdS NHs 微电极对 DA 表现出显著的负响应，从而能够开发微型自供电 PEC 器件，用于在人唾液中进行精确定量。此外，利用密度泛函理论计算阐明了 DA 的结构特征和 CdS 的缺陷态，从而为优化 DA 的聚合过程奠定了重要的理论基础。本研究为开发具有高能量转换效率的 PEC 半导体提供了一种潜在的工程方法，并提出了一种用于设计敏感测试策略的新概念。
